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Ultra‐Low Loading Pt/CeO 2 Catalysts: Ceria Facet Effect Affords Improved Pairwise Selectivity for Parahydrogen Enhanced NMR Spectroscopy
Author(s) -
Song Bochuan,
Choi Diana,
Xin Yan,
Bowers Clifford R.,
HagelinWeaver Helena
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202012469
Subject(s) - selectivity , catalysis , platinum , spin isomers of hydrogen , propene , octahedron , chemistry , materials science , nanocrystal , inorganic chemistry , crystallography , nanotechnology , hydrogen , crystal structure , organic chemistry
Oxide supports with well‐defined shapes enable investigations on the effects of surface structure on metal–support interactions and correlations to catalytic activity and selectivity. Here, a modified atomic layer deposition technique was developed to achieve ultra‐low loadings (8–16 ppm) of Pt on shaped ceria nanocrystals. Using octahedra and cubes, which expose exclusively (111) and (100) surfaces, respectively, the effect of CeO 2 surface facet on Pt‐CeO 2 interactions under reducing conditions was revealed. Strong electronic interactions result in electron‐deficient Pt species on CeO 2 (111) after reduction, which increased the stability of the atomically dispersed Pt. This afforded significantly higher NMR signal enhancement in parahydrogen‐induced polarization experiments compared with the electron‐rich platinum on CeO 2 (100), and a factor of two higher pairwise selectivity (6.1 %) in the hydrogenation of propene than any previously reported monometallic heterogeneous Pt catalyst.